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Back‐contact perovskite solar cells offer a significant potential to reach high efficiency due to reduced parasitic absorption from the top surface. However, the currently reported efficiencies are considerably lower (<10%) than planar perovskite solar cells (>20%). Herein, back‐contact perovskite solar cells are fabricated to study loss mechanisms that cause low device efficiency. This work spatially resolves the short‐circuit current, open‐circuit voltage, photoluminescence quantum yield, carrier lifetime, and external quantum efficiency of the devices. The results indicate that the front surface recombination, increased nonradiative recombination at hole contact layer/perovskite interface, and the extraction barriers are three main mechanisms limiting devices from achieving high efficiencies. [ABSTRACT FROM AUTHOR]

The highest solar cell efficiencies are obtained with concentrating systems. However, these systems have two major drawbacks: solar tracking is needed and diffuse sunlight is poorly absorbed. Here, a system that overcomes both limitations is presented, by exploiting light‐induced halide segregation in mixed halide perovskite films. A monolayer of silica microspheres focuses direct sunlight in a mixed halide perovskite film below. Through light‐induced phase segregation a low bandgap region forms in the focal point. Together with funneling of excited states toward the low bandgap regions, this results in a voltage increase characteristic for concentrating systems. Diffuse sunlight is still absorbed by the high bandgap material, avoiding the loss of diffuse sunlight characteristic for conventional concentrators. The formation of low bandgap regions in the perovskite is dynamic, and can follow the position of the focus as the sun moves throughout the day, making solar tracking unnecessary. With detailed optical and electrical simulations, it is shown that this concept can lead to an increase in both voltage and current. This leads to a 6.6% absolute increase in power conversion efficiency compared to the film without microspheres. Absorption and emission measurements confirm the concentration effect, showing the promising potential for a self‐optimizing concentrating system. [ABSTRACT FROM AUTHOR]

Halide perovskites display outstanding photoluminescence quantum yield, tunable emission, and simple deposition, which make them attractive for optoelectronics. At the same time, their facile ion migration and transformation under optical, electrical, and chemical stress are seen as a major limitation. Mixed halide perovskites are particularly problematic since optical excitation can cause changes in the bandgap that are detrimental for solar cell and light‐emitting diode efficiency and stability. In this work, instead of preventing such changes, photo‐induced halide segregation in perovskites is exploited to enable responsive, reconfigurable, and self‐optimizing materials. The mixed halide perovskite film is trained to give directional light emission using a nanophotonic microlens; through a self‐optimized process of halide photosegregation, the system mimics the training stimulus. Longer training leads to more highly directional emission, while different halide migration kinetics in the light (fast training) and dark (slow forgetting) allows for material memory. This self‐optimized material performs significantly better than lithographically aligned quantum dots because it eliminates lens‐emitter misalignment and automatically corrects for lens aberrations. The system shows a combination of mimicking, improving over time, and memory, which comprise the basic requirements for learning, and allow for the intriguing prospect of intelligent optoelectronic materials. [ABSTRACT FROM AUTHOR]

Lead halide perovskites are among the most exciting classes of optoelectronic materials due to their unique ability to form high‐quality crystals with tunable bandgaps in the visible and near‐infrared using simple solution precipitation reactions. This facile crystallization is driven by their ionic nature; just as with other salts, it is challenging to form amorphous halide perovskites, particularly in thin‐film form where they can most easily be studied. Here, rapid desolvation promoted by the addition of acetate precursors is shown as a general method for making amorphous lead halide perovskite films with a wide variety of compositions, including those using common organic cations (methylammonium and formamidinium) and anions (bromide and iodide). By controlling the amount of acetate, it is possible to tune from fully crystalline to fully amorphous films, with an interesting intermediate state consisting of crystalline islands embedded in an amorphous matrix. The amorphous lead halide perovskite has a large and tunable optical bandgap. It improves the photoluminescence quantum yield and lifetime of incorporated crystalline perovskite, opening up the intriguing possibility of using amorphous perovskite as a passivating contact, as is currently done in record efficiency silicon solar cells. [ABSTRACT FROM AUTHOR]